Prussian blue analog with separated active sites to catalyze water driven enhanced catalytic treatments

Chemodynamic therapy (CDT) uses the Fenton or Fenton-like reaction to yield toxic ‧OH following H2O2 → ‧OH for tumoral therapy. Unfortunately, H2O2 is often taken from the limited endogenous supply of H2O2 in cancer cells. A water oxidation CoFe Prussian blue (CFPB) nanoframes is presented to provide sustained, external energy-free self-supply of ‧OH from H2O to process CDT and/or photothermal therapy (PTT). Unexpectedly, the as-prepared CFPB nanocubes with no near-infrared (NIR) absorption is transformed into CFPB nanoframes with NIR absorption due to the increased Fe3+-N ≡ C-Fe2+ composition through the proposed proton-induced metal replacement reactions. Surprisingly, both the CFPB nanocubes and nanoframes provide for the self-supply of O2, H2O2, and ‧OH from H2O, with the nanoframe outperforming in the production of ‧OH. Simulation analysis indicates separated active sites in catalyzation of water oxidation, oxygen reduction, and Fenton-like reactions from CFPB. The liposome-covered CFPB nanoframes prepared for controllable water-driven CDT for male tumoral mice treatments.

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All data generated that support the findings of this study are present in the article and supplementary information. The full image dataset is available from the corresponding author upon request. Besides, source data are provided with this paper.
No data was excluded from this study.
Results were replicated in independent experiments as described in manuscript. Every experiments included replicates as describe in the figure legends and experimental methods.
For in vitro study including cytotoxicity test, Live/Dead cells assay, apoptosis analysis and O2/H2O2/•OH detection, the same plates with equal seeding number of cells were randomized before treatment of different nanocubes. For in vivo study including biosafety test, biodistribution test and anti-tumor efficacy test, the experimental mice were randomized before implantation of carcinoma cells and administration of nanocubes or nanoframes.
For in vitro study, the fields of Live/Dead cells assay and O2/H2O2/•OH detection were blindly taken. For other in vivo and in vitro study, the investigators needed to know the information of treatment group and the experimental results were presented objectively using respective instruments. Note that full information on the approval of the study protocol must also be provided in the manuscript.
Antibodies were validated with different stained concentration and unstained group in tissue sections using IHC staining.
HepG2-Red-FLuc cells were obtained from PerkinElmer. A549 cells were obtained from BCRC. HUV-EC-C cell lines were obtained from ATCC.
The cell lines used were not authenticated.
The cell lines used were not tested for mycoplasma contamination.
No commonly misidentified cell lines were used in the study.
Male BALB/c mice aged 4-7 weeks were obtained from the Laboratory Animal Center at National Cheng Kung University, Taiwan. NOD. CB17-Prkdcscid/NcrCrl (NOD-SCID) mice (6-8 weeks, male) were obtained from Labratory Animal Center, Kaohsiung Chang Gung Memorial Hospital, which is awarded Association for Assessment and Accreditation of Laboratory Animal Care International (AAALAC) accreditation. The experimental mice were housed in cages (three to five mice in each cage) at 22~23°C and 55 ± 10% humidity with 13 hr /11 hr light/dark cycle.
No wild animals were used in this study.
The sex difference was not important for in vivo experiments including biosafety study, biodistribution study and antitumor efficacy study. Therefore, in this study we performed the all animal experiments using male mice.
There are no samples collected from the field in this study.
Animal care was provided in accordance with the Laboratory Animal Welfare Act and the Guide for the Care and Use of Laboratory Animals and approved by the Institutional Animal Care and Use Committee of Kaohsiung Chang Gung Memorial Hospital (KCGMH). All animal treatments and surgical procedures were performed in accordance with the guidelines of KCGMH Laboratory Animal Center (IACUC NO. 2021031802).